Orochimaru - Naruto - I simply admire his devotion in gaining power.
Zabuza - Naruto - Somehow I feel like I can totally relate to him.
Uchiha Itachi - Naruto - My favourite one, he's powerful and always calm (when he's not killing people of course).
Android #18 & 17 - Dragon Ball - They were so cool when I was a kid, still on my list as favourite villains ^^
Pretty much all I can think of now.
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